Boron nitride (BN) is a chemically inert non-oxide ceramic material which has a multiplicity of uses based upon its electrical insulating property, corrosion resistance, high thermal conductivity and lubricity. A preferred use is as a filler material additive to a polymeric compound for use in semiconductor manufacture as an encapsulating material or to form a low viscosity thermosetting adhesive or in formulating a cosmetic material. As presently manufactured boron nitride is formed by a high temperature reaction between inorganic raw materials into a white powder composition of BN particles having an hexagonal structure similar to graphite in a platelet morphology. The platelet morphology is for many applications undesirable and of limited utility. A conventional powder composition of BN particles has the physical attributes of flour in terms of its inability to flow. Accordingly, when added as a filler to a polymer a blended material is formed having poor rheological properties and at loaded concentrations above 30 wt. % BN the blended material is so viscous that it is difficult to dispense from a mechanical dispenser such as a syringe. The physical characteristics of the filled polymer are enhanced at loading concentrations above 30 wt. % BN. Accordingly, a powder composition of BN particles with an improved rheology for use as a filler at high loading concentrations would be desirable.
The surface morphology and shape of conventional platelet BN particles are modified in accordance with the present invention to form boron nitride agglomerated particles bound by an organic binder such that when filled into a polymeric compound at loading levels between 30 to 50 wt. % BN the viscosity of the filled composition remains below 300 cp and preferably below a viscosity of 250 cp.
In accordance with the present invention, a low viscosity composition of spherically shaped agglomerated particles of boron nitride can be formed by spray drying an aqueous slurry composed of boron nitride particles of random irregular shape in combination with an organic binder and a base adapted to maintain the pH of the slurry above about 7.3 and optimally above a pH of 7.5, at a sustained elevated temperature into a dry powder composition of spherically shaped BN agglomerated particles with the concentration of the organic binder in the slurry adjusted to at least above about 1.8 wt. % of the slurry to form a residue of organic binder and/or a decomposition layer from said organic binder on said particles for modifying the surface viscosity of the composition without degrading the physical properties attributable to boron nitrate such as high thermal conductivity.
Each BN particle in the composition of the present invention represents a composite agglomerate of non-spherical BN particles bound together by an organic binder in a generally spherical geometry. The diameter of each spherically shaped BN particle formed by the spray drying method of the present invention may vary in size over a relatively wide size distribution of sizes but may be controlled so that the majority of particles and up to about 98% of the BN particles have a minimum diameter above one micron and preferably a minimum diameter above about 5 microns. The size distribution of the BN particles may extend to a maximum diameter of about 275 microns. Although the size distribution is relatively wide the BN particles have an average size which falls into a much narrower size range between about 10 microns and 150 microns in diameter and can be adjusted to form an even narrower size range by adjustment of the physical parameters of the spray drying operation and/or the initial size of the non-spherical particles of BN in the slurry. Accordingly, the size of the spherical BN agglomerated particles formed in the spray drying process of the present invention can be controllably varied over of a preferred range of from as low as 1 micron in diameter to a preferred maximum diameter of about 75 microns so as to accommodate a variety of end uses.
The spherical shape of the BN particles formed in accordance with the present invention and the weight concentration of organic binder in the slurry controls the degree to which the particles flow and, in turn, the viscosity of the polymeric compound into which the particles are loaded. The ability to xe2x80x9cflowxe2x80x9d is an essential characteristic of the spray dried BN material when used as a low viscosity filler. The degree to which a material can xe2x80x9cflowxe2x80x9d is readily measurable as is well known to those skilled in the art. In contrast, a powder composition of conventional non-spherical BN is unable to flow and inhibits the flow characteristic of the filled polymer. The standard used in the present invention to establish the existence or non-existence of a flowable material is the ASTM B213-77 hall flow standard as is well known to those skilled in the art. In the present invention, it is essential to be able to load the BN spray dried particles into a polymeric compound at loading levels of above at least 30 wt. % BN and preferably between about 35 to 50 wt. % BN without increasing the viscosity of the blend above about 250cp. The BN particles can be loaded into any polymer selected from the group consisting of a polyester, a polymide or an epoxy.
A low viscosity BN filled composition is formed in accordance with the method of the present invention comprising the steps of: forming an aqueous slurry composed of irregular non-spherically shaped BN particles, water, an organic binder and a base for maintaining the pH of the slurry at a pH above 7.3, adjusting the concentration of organic binder to a minimum level above about 1.8 wt. % of the slurry and preferably above about 2 wt. %; spray drying the aqueous slurry into a powder consisting of agglomerated BN particles of generally spherical shape and adding the powder as a filler into a polymeric compound at a loading level of between 30 to 50 wt. % BN.